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1.
J Colloid Interface Sci ; 608(Pt 3): 2246-2256, 2022 Feb 15.
Artículo en Inglés | MEDLINE | ID: mdl-34758919

RESUMEN

Supercapacitor with high storage capacity and small volumes are the development trends of miniaturization and portable energy storage systems. Herein, we design a novel self-supporting P-doped carbon nanotube (P-CNT) intercalating NiCo2O4/CoP core-shell polyhedron film. P-CNT is an ideal substrate with high electrical conductivity and interconnected porous architecture, which can enable the electrons transport to an external circuit from the electroactive component. NiCo2O4/CoP core-shell fluffy polyhedrons are derived from metal-organic frameworks with rich oxygen vacancies and abundant characteristics of pseudocapacitance, as well as better wettability. The self-supporting composite film readily achieves an ultra-high gravimetric and volumetric capacitance of 1918.4 F g-1 and 1074.3 F cm-3 at 1 A g-1. Accordingly, as-assembled hybrid supercapacitors using two binder-free electrodes, i.e., a self-supporting composite film as the positive electrode and P-doped CNT integrating graphene film as the negative electrode, harvest a remarkable gravimetric/volumetric energy density of 68.6 W h kg-1 (41.8 W h L-1) at 800 W kg-1 (488 W L-1). Our work suggests that the rational-designed NiCo2O4/CoP@P-CNTs electrode is a competitive candidate for designing next-generation supercapacitors with high volumetric energy density.

2.
J Colloid Interface Sci ; 602: 627-635, 2021 Nov 15.
Artículo en Inglés | MEDLINE | ID: mdl-34147753

RESUMEN

Recently, carbon nanotubes (CNT)-based interconnected architectures exhibit promising prospects in supercapacitors due to their flexibility and high electrical conductivity. Herein, a three-dimensional (3D) interconnected network structure combined with conductive carbon nanotubes interpenetrating MOFs-derived Co-Ni-S composite spheres (Co-Ni-S/CNTs) was synthesized. Such 3D interconnected architecture significantly leads to a favorable electronic structure, fast charge-transfer capacity, and more pseudocapacitive. The Co-Ni-S/CNTs-based hybrid electrode exhibits an extraordinary specific capacitance of 540.6C g-1 at 1 A g-1 and competitive rate performance (capacity retention rate of 69.9% when the current density increases to 10 times). Subsequently, a hybrid supercapacitor is assembled using Co-Ni-S/CNTs as the positive electrode and commercial activated carbon as negative electrode. The device delivers a high energy density of 63.5 W h kg-1 at 800 W kg-1 and keeps 83.0% initial capacitance retention after 10,000 cycles. The encouraging performances demonstrate the significant contribution of the 3D interconnected architecture for the future energy storage.


Asunto(s)
Nanotubos de Carbono , Capacidad Eléctrica , Conductividad Eléctrica , Electrodos , Electrónica
3.
J Colloid Interface Sci ; 601: 793-802, 2021 Nov.
Artículo en Inglés | MEDLINE | ID: mdl-34102407

RESUMEN

Multi-dimensional metal oxides have become a promising alternative electrode material for supercapacitors due to their inherent large surface area. Herein, P-doped NiCo2O4/NiMoO4 multi-dimensional nanostructures are synthesized on carbon clothes (CC) with a continuous multistep strategy. Especially, P has the best synergistic effect with transition metals, such as optimal deprotonation energy and OH- adsorption energy, which can further enhance electrochemical reaction activity. For the above reasons, the P-NiCo2O4/NiMoO4@CC electrode exhibits an ultra-high specific capacitance of 2334.0 F g-1 at 1 A g-1. After 1500 cycles at a current density of 10 A g-1, its specific capacity still maintains 93.7%. Besides, a P-NiCo2O4/NiMoO4@CC//activated carbon device (hybrid supercapacitor or device) was also prepared with a maximum energy density of 45.1 Wh kg-1 at a power density of 800 W kg-1. In particular, the capacity retention rate is still 89.97% after 8000 cycles due to its excellent structural stability. Our work demonstrates the vast potential of multi-dimensional metal oxides in energy storage.

4.
mBio ; 11(3)2020 06 02.
Artículo en Inglés | MEDLINE | ID: mdl-32487761

RESUMEN

The heterochromatin environment plays a central role in silencing genes associated with the malaria parasite's development, survival in the host, and transmission to the mosquito vector. However, the underlying mechanism regulating the dynamic chromatin structure is not understood yet. Here, we have uncovered that Plasmodium falciparum Rrp6, an orthologue of eukaryotic RNA exosome-associated RNase, controls the silencing of heterochromatic genes. PfRrp6 knockdown disrupted the singular expression of the GC-rich ncRNA RUF6 family, a known critical regulator of virulence gene expression, through the stabilization of the nascent transcripts. Mechanistic investigation showed that the accumulation of the multiple RUF6 ncRNAs triggered local chromatin remodeling in situ, which activated their adjacent var genes. Strikingly, chromatin isolation by RNA purification analysis (ChIRP-seq) revealed that a remarkable RUF6 ncRNA had interacted with distal heterochromatin regions directly and stimulated a global derepression effect on heterochromatic genes, including all variant gene families and the sexual commitment-associated regulator ap2-g gene. Collectively, Rrp6 appears to conduct the epigenetic surveillance of heterochromatic gene expression through controlling RUF6 levels, thereby securing antigenic variation and sexual commitment of malaria parasites during the infection of the host.IMPORTANCE Malaria remains a major public health and economic burden. The heterochromatin environment controls the silencing of genes associated with the fate of malaria parasites. Previous studies have demonstrated that a group of GC-rich ncRNAs (RUF6) is associated with the mutually exclusive expression of var genes, but the underlying mechanisms remain elusive. Here, through a series of genetic manipulation and genome-wide multiomics analysis, we have identified the plasmodial orthologue of RNA exosome-associated Rrp6 as an upstream regulator of RUF6 expression and revealed that the dysregulation of RUF6 upon Rrp6 knockdown triggered local chromatin alteration, thereby activating most heterochromatic genes via direct interaction of RUF6 and distal gene loci. This finding not only uncovered the in-depth mechanism of RUF6-mediated regulation of heterochromatic genes but also identified Rrp6 as a novel regulator of gene expression in human malaria parasites, which provides a new target for developing intervention strategies against malaria.


Asunto(s)
Regulación de la Expresión Génica , Silenciador del Gen , Plasmodium falciparum/genética , Proteínas Protozoarias/genética , ARN no Traducido/metabolismo , Expresión Génica , Heterocromatina , Humanos , Proteínas Protozoarias/metabolismo , ARN no Traducido/genética , Virulencia/genética
5.
J Am Chem Soc ; 141(9): 4130-4136, 2019 Mar 06.
Artículo en Inglés | MEDLINE | ID: mdl-30793890

RESUMEN

The pore space partition (PSP) approach has been employed to realize a novel porous MOF (FJU-90) with dual functionalities for the challenging C2H2/CO2 separation under ambient conditions. By virtue of a triangular ligand (Tripp = 2,4,6-tris(4-pyridyl)pyridine), the cylindrical channels in the original FJU-88 have been partitioned into uniformly interconnected pore cavities, leading to the dramatically reduced pore apertures from 12.0 × 9.4 to 5.4 × 5.1 Å2. Narrowing down the pore sizes, the resulting activated FJU-90a takes up a very large amount of C2H2 (180 cm3 g-1) but much less of CO2 (103 cm3 g-1) at 298 K and 1 bar, demonstrating it to be the best porous MOF material for this C2H2/CO2 (50%:50%) separation in terms of the C2H2 gravimetric productivity. IAST calculations, molecular modeling studies, and simulated and experimental breakthrough experiments comprehensively demonstrate that the pore space partition strategy is a very powerful approach to constructing MOFs with dual functionality for challenging gas separation.

6.
ACS Appl Mater Interfaces ; 10(36): 30912-30918, 2018 Sep 12.
Artículo en Inglés | MEDLINE | ID: mdl-30124288

RESUMEN

Although supramolecular isomerism in metal-organic frameworks (MOFs) would offer a favorable platform for in-depth exploring their structure-property relationship, the design and synthesis of the isomers are still rather a challenging aspect of crystal engineering. Here, a pair of supramolecular isomers of Co(II)-based MOFs (FJU-88 and FJU-89) can be directionally fabricated by rational tuning the additives. In spite of the fact that the isomers have the similar Co3 secondary building units and organic linkers, they adopt distinct networks with acs and snw topologies, respectively, which derive from the conformational flexibility of the organic ligands. It is noteworthy that the porous structure of FJU-88 would be collapsed after removal of the solvent from the pores. But FJU-89a shows permanent porosity accompanied with unusual hierarchical micro- and mesopores and superior gas selective adsorption performance. In addition, FJU-89a can efficiently trap C2H2 from C2H2/CO2 and C2H2/CH4 mixture gases through fixed-bed dynamic breakthrough experiments.

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